Transition between growth of dense and porous films: theory of dual-layer SEI

Kolzenberg, Lars von; Werres, Martin; Tetzloff, Jonas; Horstmann, Birger

doi:10.1039/d2cp00188h

Cited by 13 publications

(12 citation statements)

References 74 publications

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“…(2) For smaller stripping current densities, notches can more easily occur and are thus more likely to occur. As discussed above, local variations play a lesser role at higher stripping current densities. − Thus, higher stripping current densities can mitigate the emergence of notches and thus can lead to less isolated lithium.…”

Section: Results and Discussionmentioning

confidence: 97%

“…For this simulation, we choose the stripping current density to be J = J 0 . In this scenario, the local variations of interfacial tension become irrelevant and the local stripping current density variations are negligible. − Therefore, the lithium–SEI bond breaking occurs homogeneously; see Figure b,c. During stripping, the whisker is thinned until it is dissolved, as depicted in Figure d,e.…”

Section: Results and Discussionmentioning

confidence: 99%

“…Unlike canonical phase-field models, where the solid/liquid phases are captured by a phase parameter and a diffuse edge, 68−75 we assume a sharp edge and only track the surface of the whisker. 50,51 The dynamics of the whisker dissolution can then be described by the propagation of the surface points ξ which move perpendicular to the surface:…”

Section: Methodsmentioning

confidence: 99%

“…Unlike canonical phase-field models, where the solid/liquid phases are captured by a phase parameter and a diffuse edge, − we assume a sharp edge and only track the surface of the whisker. , The dynamics of the whisker dissolution can then be described by the propagation of the surface points ξ which move perpendicular to the surface: ∂ r ( ξ ) ∂ t = ż ṙ 2 + ż 2 · V normalM F · J ( ξ ) ∂ z ( ξ ) ∂ t = − ṙ ṙ 2 + ż 2 · V normalM F · J ( ξ ) Here, r ̇ = ∂ r /∂ξ, z ̇ = ∂ z /∂ξ, V M = 13.02 × 10 –6 m 3 mol –1 is the molar volume of lithium, F is the Faraday constant, and J (ξ) is the electrical current density, given by the Butler–Volmer expression J ( ξ ) = J 0 [ e − F normalΔ normalΦ / 2 R T ...…”

Section: Methodsmentioning

confidence: 99%

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Origin of Heterogeneous Stripping of Lithium in Liquid Electrolytes

Werres

Jia

et al. 2023

ACS Nano

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Lithium metal batteries suffer from low cycle life. During discharge, parts of the lithium are not stripped reversibly and remain isolated from the current collector. This isolated lithium is trapped in the insulating remaining solid-electrolyte interphase (SEI) shell and contributes to the capacity loss. However, a fundamental understanding of why isolated lithium forms and how it can be mitigated is lacking. In this article, we perform a combined theoretical and experimental study to understand isolated lithium formation during stripping. We derive a thermodynamic consistent model of lithium dissolution and find that the interaction between lithium and SEI leads to locally preferred stripping and isolated lithium formation. Based on a cryogenic transmission electron microscopy (cryo TEM) setup, we reveal that these local effects are particularly pronounced at kinks of lithium whiskers. We find that lithium stripping can be heterogeneous both on a nanoscale and on a larger scale. Cryo TEM observations confirm our theoretical prediction that isolated lithium occurs less at higher stripping current densities. The origin of isolated lithium lies in local effects, such as heterogeneous SEI, stress fields, or the geometric shape of the deposits. We conclude that in order to mitigate isolated lithium, a uniform lithium morphology during plating and a homogeneous SEI are indispensable.

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Section: Results and Discussionmentioning

confidence: 97%

Section: Results and Discussionmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

See 2 more Smart Citations

Origin of Heterogeneous Stripping of Lithium in Liquid Electrolytes

Werres

Jia

et al. 2023

ACS Nano

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show abstract

“…Despite a lot of effort that has been going into the theoretical and experimental investigation of the SEI for many years, the SEI is still not fully understood [5,6,7]. This results from the complexity of the SEI due to the variety of organic and inorganic SEI components [8,9,10], mixed layered and mosaic SEI structures [11,12,13,14,15], a heterogeneous SEI morphology [16,17,18], and the contribution of different SEI formation reactions to the evolution of the SEI [19,20,21,22,23].…”

Section: Introductionmentioning

confidence: 99%